A gauge-invariant density matrix approach is presented to describe the non-equilibrium dynamics of multiband superconductors after photo-excitation. The derived gauge-invariant Bloch equations extend the Anderson pseudo-spin precession model by fully incorporating the center-of-mass motion of Cooper pairs. We also describe lightwave propagation effects inside a superconducting film by including the self-consistent interaction of the photo-excited superconducting system with the propagating electromagnetic field inside the superconductor using Maxwell's equations.
Magnetically doped topological insulators (TIs) attract a great deal of interest for both fundamental scientific studies and potential applications. These systems are promising for the realization of quantum anomalous Hall effect, and more generally, for the potentially controllable magnetism, which can underlay many useful technological applications. Here, we reveal the first photoinduced magnetization dynamics in a 40 nm thin film of magnetically doped TIs, CrxBi2-xTe3 with x=0.29 using femtosecond time-resolved magneto-optical Kerr effect (MOKE) spectroscopy. The ultrafast spin dynamics of the sample at low temperature 5 K is characterized by two demagnetization dynamics, attributed to spin-spin (~0.5 ps) and spin-phonon (~10 ps) scatterings, respectively, followed by a slow recovery process with 100s of ps time scale. While it gets faster at elevated temperature and finally vanishes above ~ 90 K, much higher than the reported Curie temperature Tc~23.8 K, due to strong Van Vleck magnetic susceptibility in the magnetically doped TIs system, distinct from the case of GaMnAs. In addition to providing implications for deeper understanding of spin dynamics in magnetically doped TI systems, the study will potentially benefit the development of magnetic TIs-based spintronic devices.
We use a non-equilibrium many-body theory that engages the elements of transient coherence, correlation, and nonlinearity to describe changes in the magnetic and electronic phases of strongly correlated systems induced by femtosecond nonlinear photoexcitation. Using a generalized tight–binding mean field approach based on Hubbard operators and including the coupling of the laser field, we describe a mechanism for simultaneous insulator–to–metal and anti- to ferro–magnetic transition to a transient state triggered by non–thermal ultrafast spin and charge coupled excitations. We demontrate, in particular, that photoexcitation of composite fermion quasiparticles induces quasi-instantaneous spin canting that quenches the energy gap of the antiferromagnetic insulator and acts as a nonadiabatic “initial condition” that triggers non-thermal lattice dynamics leading to an insulator to metal and antiferromagnetic (AFM) to ferromagnetic (FM) transitions. Our theoretical predictions are consistent with recent ultrafast pump-probe spectroscopy experiments that revealed a magnetic phase transition during 100fs laser pulse photoexcitation of the CE–type AFM insulating phase of colossal magnetoresistive manganites. In particular, experiment observes two distinct charge relaxation components, fs and ps, with non- linear threshold dependence at a pump fluence threshold that coincides with that for femtosecond magnetization photoexcitation. Our theory attributes the correlation between femtosecond spin and charge nonlinearity leading to transition in the magnetic and electronic state to spin/charge/lattice coupling and laser-induced quantum spin canting that accompanies the driven population inversion between two quasi–particle bands with different properties: a mostly occupied polaronic band and a mostly empty metallic band, whose dispersion is determined by quantum spin canting.
How photoexcitations evolve in time into Coulomb-bound electron and hole pairs, called excitons, and unbound charge carriers is a key cross-cutting issue in photovoltaic and optoelectronic technologies. Until now, the initial quantum dynamics following photoexcitation remains elusive in the organometal halide perovskite system. Here we reveal excitonic Rydberg states with distinct formation pathways by observing the multiple resonant internal quantum transitions using ultrafast terahertz quasi-particle transport. Nonequilibrium emergent states evolve with a complex co-existence of excitons, unbound carriers and phonons, where a delayed buildup of excitons under on- and off-resonant pumping conditions allows us to distinguish between the loss of electronic coherence and hot state cooling processes. The terahertz transport with rather long dephasing time and scattering processes due to discrete terahertz phonons in perovskites are distinct from conventional photovoltaic materials. In addition to providing implications for ultrafast coherent transport, these results break ground for a perovskite-based device paradigm for terahertz and coherent optoelectronics.
Many-body correlation effects in complex quantum systems often lead to phase transitions that bear great technological potential. However, the underlying microscopic driving mechanisms or even the quantum-mechanical properties of the novel ground state often remain elusive. Here we employ phase-locked ultrabroadband terahertz (THz) pulses to disentangle two coexisting orders in the charge density wave phase 1T-TiSe2 via their individual non-equilibrium multi- THz dynamics. Furthermore, we demonstrate that few-cycle THz pulses can project out the matter part of a transient cold exciton-polariton condensate, providing novel insights into the very nature of this macroscopic quantum state.
The technological demand to push the gigahertz switching speed limit of today’s magnetic memory/logic devices into the terahertz (1THz=1ps−1) regime underlies the entire field of spin–electronics and integrated multi- functional devices. This challenge is met by all–optical magnetic switching based on coherent spin manipulation By analogy to femto–chemistry and photosynthetic dynamics where photo-products of chemical/biochemical re- actions can be influenced by creating suitable superpositions of molecular states, femtosecond (fs) laser–excited coherence between spin/orbital/charge states can switch magnetic orders, by “suddenly” breaking the delicate balance between competing phases of correlated materials, e.g., the colossal magneto–resistive (CMR) manganites suitable for applications. Here we discuss femtosecond (fs) all-optical switching from antiferro- to ferromagnetic ordering via establishment of a magnetization increase within ∼100 fs, while the laser field still interacts with the system. Such non-equilibrium ferromagnetic correlations arise from quantum spin–flip fluctuations corre- lated with coherent superpositions of electronic states. The development of ferromagnetic correlations during the fs laser pulse reveals an initial quantum coherent regime of magnetism, clearly distinguished from the pi- cosecond lattice-heating regime characterized by phase separation. We summarize a microscopic theory based on density matrix equations of motion for composite fermion Hubbard operators, instead of bare electrons, that take into account the strong spin and charge local correlations. Our work merges two fields, femto-magnetism in metals/band insulators and non–equilibrium phase transitions of strongly correlated electrons, where local interactions exceeding the kinetic energy produce a complex balance of competing orders.
Characteristic low-threshold polariton lasing of organic and inorganic microcavity systems can only be achieved with
efficient population of the lower polariton ground state. In this regard, the key role undertaken by vibronic replicas and
molecular phonon it has been shown experimentally and theoretically predicted by various works. We report here, direct
observation of critical enhancement of polariton population density in strongly coupled J-aggregate based organic
microcavities. The process highlighted in our study is manifested by discrete maxima of the angular-resolved
photoluminescence intensity and interpreted by the mediation of molecular vibrations quanta characteristic of the active
material. By measuring the reduced time scale of vibrations driven relaxation dynamics, manifested by sub 100fs buildup
times, we emphasized the efficiency of the mechanism to overcome losses channel in disordered J-aggregate systems.
Hence, the realization of amplified polariton population with improved relaxation rates paves the way for the observation
of low threshold lasing, primary step for developing room temperature organic laser sources and ultra-fast optoelectronic
devices with less fabrication complexity than their crystalline counterparts.
We report a femtosecond response in photoinduced magnetization rotation in the ferromagnetic semiconductor
GaMnAs, which allows for detection of a four-state magnetic memory at the femtosecond time scale. The
temporal profile of this cooperative magnetization rotation exhibits a discontinuity that reveals two distinct
temporal regimes, marked by the transition from a highly non-equilibrium, carrier-mediated regime within the
first 200 fs, to a thermal, lattice-heating picosecond regime.
We report comprehensive temperature and photoexcitation intensity dependent studies of the photoinduced
magnetization precession in Ga1-xMnxAs (x = 0.035) by time-resolved Kerr rotation measurements. We observe coherent
oscillations of local Mn spins triggered by an ultrafast photo-induced reorientation of the easy axis due to changes in the
magnetic anisotropy. The amplitude saturation of these oscillations above certain pump intensity is indicative of
stabilization of the magnetic easy axis orientation on temperatures above ~Tc/2. We find that the observed magnetization
precession damping (Gilbert damping) is strongly dependent on pump laser intensity, but largely independent of ambient
temperature.
We discuss the role of many-body spin correlations in nonlinear optical response of a Fermi sea system with a deep impurity level. Due to the Hubbard repulsion between electrons at the impurity, the optical transitions between the impurity level and the Fermi sea states lead to an optically-induced Kondo effect. In particular, the third- order nonlinear optical susceptibility logarithmically diverges at the absorption threshold. The shape of the pump- probe spectrum is governed by the light-induced Kondo temperature, which can be tuned by varying the intensity and frequency of the pump optical field. In the Kondo limit, corresponding to off-resonant pump excitation, the nonlinear absorption spectrum exhibits a narrow peak below the linear absorption onset.
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